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Dynamics of a Laser-Irradiated Adatom.
STATE UNIV OF NEW YORK AT BUFFALO DEPT OF CHEMISTRY
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The dynamics of an adsorbed atom irradiated by an IR laser in resonance with a single pair of states of the vibrational adbond is studied. Using a non-perturbative treatment for the laser adbond interaction, a master equation is derived, which governs the time evolution of the populations of the laser dressed states of the adbond. The effect of resonant heating and laser induced desorpton, as an example of a possible laser induced surface process, is discussed. A master equation for the time evolution of the populations of the laser dressed states of the reduced density matrix of the adbond is derived. The transitions between the states can be interpreted as phonon transitions between the dressed levels of the adbond. Stimulated radiative transitions are incorporated in the transformation to dressed states. The phonon transitions between the adbond states give rise to an energy flow from the laser into the substrate. Even in the steady state where the level populations are time independent the energy flow assumes a non-zero value.
APPROVED FOR PUBLIC RELEASE